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Interatomic Coulombic decay in small helium clusters.

Sévan Kazandjian1, Max Kircher2, Gregor Kastirke2

  • 1Sorbonne Universite, CNRS, Laboratoire de Chimie Physique Matiere et Rayonnement, UMR 7614, F-75005 Paris, France. nicolas.sisourat@sorbonne-universite.fr.

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Summary
This summary is machine-generated.

Interatomic Coulombic decay (ICD) in helium clusters is faster for larger clusters due to more decay channels and closer atoms. This ultrafast process influences ion kinetic energies, revealing cluster size distributions.

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Area of Science:

  • Atomic and Molecular Physics
  • Quantum Chemistry
  • Cluster Science

Background:

  • Interatomic Coulombic decay (ICD) is a non-radiative process where energy transfers between excited atoms, causing ionization.
  • In helium clusters, ICD can occur after ionization and excitation of a single helium atom, leading to a Coulomb explosion.
  • Understanding ICD dynamics in small helium clusters is crucial for interpreting experimental observations.

Purpose of the Study:

  • To theoretically investigate Interatomic Coulombic decay (ICD) in small helium clusters (2-7 atoms).
  • To compare theoretical findings with experimental coincidence measurements on helium clusters of varying mean sizes.
  • To elucidate the influence of cluster size on ICD rates and decay dynamics.

Main Methods:

  • Theoretical investigation of ICD in helium clusters ranging from 2 to 7 atoms.
  • Comparison of theoretical predictions with experimental coincidence measurements.
  • Analysis of kinetic-energy distributions of helium ions resulting from ICD and frustrated Coulomb explosions.

Main Results:

  • ICD rates increase with cluster size due to a higher number of decay channels and reduced interatomic distances.
  • A prediction for the lifetime of the excited helium dimer is provided.
  • Kinetic-energy distributions reveal charge exchange processes (frustrated Coulomb explosion), which become more probable in larger clusters.

Conclusions:

  • ICD is a significant decay pathway in small helium clusters, with rates strongly dependent on cluster size.
  • The observed kinetic-energy distributions are characteristic of the cluster size distribution and provide insights into frustrated Coulomb explosion dynamics.
  • Theoretical modeling successfully reproduces experimental findings, validating the understanding of ICD in helium clusters.